DEVELOPMENT OF IMPROVED CATALYSTS FOR THE SELECTIVE CATALYTIC REDUCTION OF NITROGEN OXIDES WITH HYDROCARBONS

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Significant work has been done by the investigators on the cerium oxide-copper oxide based sorbent/catalysts for the combined removal of sulfur and nitrogen oxides from the flue gases of stationary sources. A relatively wide temperature window was established for the use of alumina-supported cerium oxide-copper oxide mixtures as regenerable sorbents for SO{sub 2} removal. Evaluation of these sorbents as catalysts for the selective reduction of NO{sub x} gave promising results with methane. Since the replacement of ammonia by methane is commercially very attractive, in this project, it was planned to investigate the effect of promoters on the activity and selectivity ...
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Description

Significant work has been done by the investigators on the cerium oxide-copper oxide based sorbent/catalysts for the combined removal of sulfur and nitrogen oxides from the flue gases of stationary sources. A relatively wide temperature window was established for the use of alumina-supported cerium oxide-copper oxide mixtures as regenerable sorbents for SO{sub 2} removal. Evaluation of these sorbents as catalysts for the selective reduction of NO{sub x} gave promising results with methane. Since the replacement of ammonia by methane is commercially very attractive, in this project, it was planned to investigate the effect of promoters on the activity and selectivity of copper oxide/cerium oxide-based catalysts and to obtain data on the reaction mechanism for the SCR with methane. The investigation of the reaction mechanism will help in the selection of promoters to improve the catalytic activity and selectivity of the sorbents in the SCR with methane. This will result in new catalyst formulations. The last component of the project involves our industrial partner TDA Research, and the objective is to evaluate long- term stability and durability of the prepared sorbent/catalysts. In the second year of the project, the catalysts were investigated for their SCR activity with methane in a microreactor setup and also, by the temperature-programmed desorption (TPD) technique. The results from the SCR experiments indicated that manganese is a more effective promoter than rhodium on the supported copper oxide-ceria catalysts under study; the effectiveness of the promoter increases with the increase in Ce/Cu ratio. The TPD profiles of the unpromoted catalyst (Cu/Ce=3) is different than those promoted with 0.1% rhodium. In the current reporting period, the screening of the promoted catalysts were completed, sufficient amount of the selected catalysts were prepared and delivered to TDA for long term deactivation testing.

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